The paper proposes a biomass cross-upgrading process that combines hydrothermal carbonization and pyrolysis to produce high-quality blast furnace injection fuel.The results showed that after upgrading,the volatile con...The paper proposes a biomass cross-upgrading process that combines hydrothermal carbonization and pyrolysis to produce high-quality blast furnace injection fuel.The results showed that after upgrading,the volatile content of biochar ranged from 16.19%to 45.35%,and the alkali metal content,ash content,and specific surface area were significantly reduced.The optimal route for biochar pro-duction is hydrothermal carbonization-pyrolysis(P-HC),resulting in biochar with a higher calorific value,C=C structure,and increased graphitization degree.The apparent activation energy(E)of the sample ranges from 199.1 to 324.8 kJ/mol,with P-HC having an E of 277.8 kJ/mol,lower than that of raw biomass,primary biochar,and anthracite.This makes P-HC more suitable for blast furnace injection fuel.Additionally,the paper proposes a path for P-HC injection in blast furnaces and calculates potential environmental benefits.P-HC of-fers the highest potential for carbon emission reduction,capable of reducing emissions by 96.04 kg/t when replacing 40wt%coal injec-tion.展开更多
In order to obtain liquefied products with higher yields of aromatic molecules to produce mesophase pitch,a good understanding of the relevant reaction mechanisms is required.Reactive molecular dynamics simulations we...In order to obtain liquefied products with higher yields of aromatic molecules to produce mesophase pitch,a good understanding of the relevant reaction mechanisms is required.Reactive molecular dynamics simulations were used to study the thermal reactions of pyrene,1-methylpyrene,7,8,9,10-tetrahydrobenzopyrene,and mixtures of pyrene with 1-octene,cyclohexene,or styrene.The reactant conversion rates,reaction rates,and product distributions were calculated and compared,and the mechanisms were analyzed and discussed.The results demonstrated that methyl and naphthenic structures in aromatics might improve the conversion rates of reactants in hydrogen transfer processes,but their steric hindrances prohibited the generation of high polymers.The naphthenic structures could generate more free radicals and presented a more obvious inhibition effect on the condensation of polymers compared with the methyl side chains.It was discovered that when different olefins were mixed with pyrene,1-octene primarily underwent pyrolysis reactions,whereas cyclohexene mainly underwent hydrogen transfer reactions with pyrene and styrene,mostly producing superconjugated biradicals through condensation reactions with pyrene.In the mixture systems,the olefins scattered aromatic molecules,hindering the formation of pyrene trimers and higher polymers.According to the reactive molecular dynamics simulations,styrene may enhance the yield of dimer and enable the controlled polycondensation of pyrene.展开更多
Hydrothermal carbonization(HTC) of lignocellulosic biomass is a promising technology for the production of carbon materials with negative carbon emissions. However, the high reaction temperature and energy consumption...Hydrothermal carbonization(HTC) of lignocellulosic biomass is a promising technology for the production of carbon materials with negative carbon emissions. However, the high reaction temperature and energy consumption have limited the development of HTC technology. In conventional batch reactors, the temperature and pressure are typically coupled at saturated states. In this study, a decoupled temperature and pressure hydrothermal(DTPH) reaction system was developed to decrease the temperature of the HTC reaction of lignocellulosic biomass(rice straw and poplar leaves). The properties of hydrochars were analyzed by scanning electron microscopy(SEM), Fourier transform infrared(FTIR) spectroscopy, X-ray photoelectron spectroscopy(XPS), Raman spectroscopy, X-ray diffraction(XRD), thermogravimetric analyzer(TGA), etc. to propose the reaction mechanism. The results showed that the HTC reaction of lignocellulosic biomass could be realized at a low temperature of 200℃ in the DTPH process, breaking the temperature limit(230℃) in the conventional process. The DTPH method could break the barrier of the crystalline structure of cellulose in the lignocellulosic biomass with high cellulose content, realizing the carbonization of cellulose and hemicellulose with the dehydration, unsaturated bond formation, and aromatization. The produced hydrochar had an appearance of carbon microspheres, with high calorific values, abundant oxygen-containing functional groups, a certain degree of graphitization, and good thermal stability. Cellulose acts not only as a barrier to protect itself and hemicellulose from decomposition, but also as a key precursor for the formation of carbon microspheres. This study shows a promising method for synthesizing carbon materials from lignocellulosic biomass with a carbon-negative effect.展开更多
Propylene is a significant basic material for petrochemicals such as polypropylene,propylene oxide,etc.With abundant propane supply from shale gas,propane dehydrogenation(PDH)becomes extensively attractive as an on-pu...Propylene is a significant basic material for petrochemicals such as polypropylene,propylene oxide,etc.With abundant propane supply from shale gas,propane dehydrogenation(PDH)becomes extensively attractive as an on-purpose propylene production route in recent years.Nitrogen-doped carbon(NC)nanopolyhedra supported cobalt catalysts were synthesized in one-step of ZIF-67 pyrolysis and investigated further in PDH.XPS,TEM and N_(2) adsorption-desorption were used to study the influence of carbonization temperature on as-prepared NC supported cobalt catalysts.The temperature is found to affect the cobalt phase and nitrogen species of the catalysts.And the positive correlation was established between Co0 proportion and space time yield of propylene,indicating that the modulation of carbonization temperature could be important for catalytic performance.展开更多
Greenhouse gas emissions from waste plastics have caused global warming all over the world,which has been a central threat to the ecological environment for humans,flora and fauna.Among waste plastics,waste polyethyle...Greenhouse gas emissions from waste plastics have caused global warming all over the world,which has been a central threat to the ecological environment for humans,flora and fauna.Among waste plastics,waste polyethylene terephthalate(PET)is attractive due to its excellent stability and degradation-resistant.Therefore,merging China’s carbon peak and carbon neutrality goals would be beneficial.In this review,we summarize the current state-of-the-art of carbon emission decrease from a multi-scale perspective technologically.We suggest that the carbon peak for waste PET can be achieved by employing the closed-loop supply chain,including recycling,biomass utilization,carbon capture and utilization.Waste PET can be a valuable and renewable resource in the whole life cycle.Undoubtedly,all kinds of PET plastics can be ultimately converted into CO_(2),which can also be feedstock for various kinds of chemical products,including ethyl alcohol,formic acid,soda ash,PU,starch and so on.As a result,the closed-loop supply chain can help the PET plastics industry drastically reduce its carbon footprint.展开更多
Decarbonization is a critical issue for peaking CO_(2) emissions of energy-intensive industries,such as the iron and steel industry.The decarbonization options of China’s ironmaking and steelmaking sector were discus...Decarbonization is a critical issue for peaking CO_(2) emissions of energy-intensive industries,such as the iron and steel industry.The decarbonization options of China’s ironmaking and steelmaking sector were discussed based on a systematic three-dimensional low-carbon analysis from the aspects of resource utilization(Y),energy utilization(Q),and energy cleanliness which is evaluated by a process general emission factor(PGEF)on all the related processes,including the current blast furnace(BF)-basic oxygen furnace(BOF)integrated process and the specific sub-processes,as well as the electric arc furnace(EAF)process,typical direct reduction(DR)process,and smelting reduction(SR)process.The study indicates that the three-dimensional aspects,particularly the energy structure,should be comprehensively considered to quantitatively evaluate the decarbonization road map based on novel technologies or processes.Promoting scrap utilization(improvement of Y)and the substitution of carbon-based energy(improvement of PGEF)in particular is critical.In terms of process scale,promoting the development of the scrap-based EAF or DR-EAF process is highly encouraged because of their lower PGEF.The three-dimensional method is expected to extend to other processes or industries,such as the cement production and thermal electricity generation industries.展开更多
Hydrothermal carbonization is highly applicable to high moisture biomass upgrading due to the fact that moist-ure involved can be directly used as reaction media under the subcritical-water region.With this,value-adde...Hydrothermal carbonization is highly applicable to high moisture biomass upgrading due to the fact that moist-ure involved can be directly used as reaction media under the subcritical-water region.With this,value-added utilization of hydrochar as solid fuel with high carbon and energy density is one of the important pathways for biomass conversion.In this review,the dewatering properties of hydrochar after the hydrothermal carbonization of biowaste,coalification degree with elemental composition and evolution,pelletization of hydrochar to enhance the mechanical properties and density,coupled with the combustion properties of hydrochar biofuel were discussed with various biomass and carbonization parameters.Potential applications for the co-combustion with coal,cleaner properties and energy balance for biowaste hydrothermal carbonization were presented as well as the challenges.展开更多
High-performance carbonaceous electrode materials for supercapacitors were synthesized by subjecting corn starch to a simple molten salt activation process with K<sub>2</sub>CO<sub>3</sub> at a...High-performance carbonaceous electrode materials for supercapacitors were synthesized by subjecting corn starch to a simple molten salt activation process with K<sub>2</sub>CO<sub>3</sub> at a temperature of 850˚C. The resulting carbon material, obtained after activating for 1 hour, displayed excellent capacitive properties due to the synergistic effects of its porous structure. Utilizing these electrodes, the supercapacitor exhibited a high discharge capacitance (248 F g<sup>−1</sup> at 1 A g<sup>−1</sup>), which is 2.4 times higher than that of activated carbon without K<sub>2</sub>CO<sub>3</sub> activation. The enhancement in electrical performance was analyzed through SEM and XRD analysis, revealing that the porous and disordered structure provides a greater number of charge storage sites, resulting in improved capacitive performance.展开更多
湖泊沉积物不仅记录了湖泊演化的过程,还蕴含了丰富的碳储量。本文以青藏高原西部郭扎错407 cm长的湖芯为例,探讨了8.7 ka BP以来该湖由淡水湖演变到咸水湖的过程中,有机碳和无机碳沉积通量与储量的变化及影响因素。郭扎错无机碳沉积通...湖泊沉积物不仅记录了湖泊演化的过程,还蕴含了丰富的碳储量。本文以青藏高原西部郭扎错407 cm长的湖芯为例,探讨了8.7 ka BP以来该湖由淡水湖演变到咸水湖的过程中,有机碳和无机碳沉积通量与储量的变化及影响因素。郭扎错无机碳沉积通量范围为4.6~35.1 g·m^(-2)·a^(-1),平均值为17 g·m^(-2)·a^(-1),无机碳储量范围为2.5×10^(6)~19.1×10^(6) t/a,平均值为9.2×10^(6) t/a,无机碳总储量约为18.5×10^(9) t。有机碳沉积通量范围为1.6~7.3 g·m^(-2)·a^(-1),平均值为4.0 g·m^(-2)·a^(-1),有机碳储量范围为1.5×10^(6)~3.3×10^(6) t/a,平均值为2.2×10^(6) t/a,有机碳总储量约为1.63×10^(9) t。8.7 ka BP以来,三个不同环境演化阶段(8.7~4.0 ka BP,4.0~1.5 ka BP,以及1.5 ka BP至今)中,4.0~1.5 ka BP气候寒冷干旱,湖泊为淡水湖,但无机碳和有机碳的沉积通量和储量都表现为低值。根据碳沉积通量和储量的变化特征发现,无机碳的沉积与碳酸盐矿物成因有关,而有机碳沉积则与黏土矿物的成因有关,二者都与环境、湖水性质变化有关,其中温度对无机碳沉积通量和储量的影响大于盐度的影响,而温度对有机碳沉积通量和储量的影响小于盐度的影响。展开更多
基金the National Key R&D Program of China(No.2022YFE0208100)the National Natural Science Foundation of China(No.5274316)+1 种基金the Key Research and Development Plan of Anhui Province,China(No.202210700037)the Major Science and Technology Project of Xinjiang Uygur Autonomous Region,China(No.2022A01003).
文摘The paper proposes a biomass cross-upgrading process that combines hydrothermal carbonization and pyrolysis to produce high-quality blast furnace injection fuel.The results showed that after upgrading,the volatile content of biochar ranged from 16.19%to 45.35%,and the alkali metal content,ash content,and specific surface area were significantly reduced.The optimal route for biochar pro-duction is hydrothermal carbonization-pyrolysis(P-HC),resulting in biochar with a higher calorific value,C=C structure,and increased graphitization degree.The apparent activation energy(E)of the sample ranges from 199.1 to 324.8 kJ/mol,with P-HC having an E of 277.8 kJ/mol,lower than that of raw biomass,primary biochar,and anthracite.This makes P-HC more suitable for blast furnace injection fuel.Additionally,the paper proposes a path for P-HC injection in blast furnaces and calculates potential environmental benefits.P-HC of-fers the highest potential for carbon emission reduction,capable of reducing emissions by 96.04 kg/t when replacing 40wt%coal injec-tion.
基金financially supported by the National Natural Science Foundation of China(Approval No.42172168).
文摘In order to obtain liquefied products with higher yields of aromatic molecules to produce mesophase pitch,a good understanding of the relevant reaction mechanisms is required.Reactive molecular dynamics simulations were used to study the thermal reactions of pyrene,1-methylpyrene,7,8,9,10-tetrahydrobenzopyrene,and mixtures of pyrene with 1-octene,cyclohexene,or styrene.The reactant conversion rates,reaction rates,and product distributions were calculated and compared,and the mechanisms were analyzed and discussed.The results demonstrated that methyl and naphthenic structures in aromatics might improve the conversion rates of reactants in hydrogen transfer processes,but their steric hindrances prohibited the generation of high polymers.The naphthenic structures could generate more free radicals and presented a more obvious inhibition effect on the condensation of polymers compared with the methyl side chains.It was discovered that when different olefins were mixed with pyrene,1-octene primarily underwent pyrolysis reactions,whereas cyclohexene mainly underwent hydrogen transfer reactions with pyrene and styrene,mostly producing superconjugated biradicals through condensation reactions with pyrene.In the mixture systems,the olefins scattered aromatic molecules,hindering the formation of pyrene trimers and higher polymers.According to the reactive molecular dynamics simulations,styrene may enhance the yield of dimer and enable the controlled polycondensation of pyrene.
基金The financial support from the Key-Area Research and Development Program of Guangdong Province (2020B1111380001)the Beijing Municipal Natural Science Foundation (2222012)+1 种基金the National Natural Science Foundation of China (Grant No.52070116)the Tsinghua University-Shanxi Clean Energy Research Institute Innovation Project Seed Fund。
文摘Hydrothermal carbonization(HTC) of lignocellulosic biomass is a promising technology for the production of carbon materials with negative carbon emissions. However, the high reaction temperature and energy consumption have limited the development of HTC technology. In conventional batch reactors, the temperature and pressure are typically coupled at saturated states. In this study, a decoupled temperature and pressure hydrothermal(DTPH) reaction system was developed to decrease the temperature of the HTC reaction of lignocellulosic biomass(rice straw and poplar leaves). The properties of hydrochars were analyzed by scanning electron microscopy(SEM), Fourier transform infrared(FTIR) spectroscopy, X-ray photoelectron spectroscopy(XPS), Raman spectroscopy, X-ray diffraction(XRD), thermogravimetric analyzer(TGA), etc. to propose the reaction mechanism. The results showed that the HTC reaction of lignocellulosic biomass could be realized at a low temperature of 200℃ in the DTPH process, breaking the temperature limit(230℃) in the conventional process. The DTPH method could break the barrier of the crystalline structure of cellulose in the lignocellulosic biomass with high cellulose content, realizing the carbonization of cellulose and hemicellulose with the dehydration, unsaturated bond formation, and aromatization. The produced hydrochar had an appearance of carbon microspheres, with high calorific values, abundant oxygen-containing functional groups, a certain degree of graphitization, and good thermal stability. Cellulose acts not only as a barrier to protect itself and hemicellulose from decomposition, but also as a key precursor for the formation of carbon microspheres. This study shows a promising method for synthesizing carbon materials from lignocellulosic biomass with a carbon-negative effect.
基金This work is supported by the National Natural Science Foundation of China(Grant Nos.21802167,21961132026,92034302,21878331,91645108)the National Key Research and Development Program Nanotechnology Specific Project(No.2020YFA0210903).
文摘Propylene is a significant basic material for petrochemicals such as polypropylene,propylene oxide,etc.With abundant propane supply from shale gas,propane dehydrogenation(PDH)becomes extensively attractive as an on-purpose propylene production route in recent years.Nitrogen-doped carbon(NC)nanopolyhedra supported cobalt catalysts were synthesized in one-step of ZIF-67 pyrolysis and investigated further in PDH.XPS,TEM and N_(2) adsorption-desorption were used to study the influence of carbonization temperature on as-prepared NC supported cobalt catalysts.The temperature is found to affect the cobalt phase and nitrogen species of the catalysts.And the positive correlation was established between Co0 proportion and space time yield of propylene,indicating that the modulation of carbonization temperature could be important for catalytic performance.
基金The authors acknowledge the financial support provided by the Key R&D Program of Shaanxi Province(No.2022SF-168)Xi’an Programs for Science and Technology Plan(Nos.2020KJRC0090 and 21XJZZ0045)+5 种基金Xi’an Beilin District Programs for Science and Technology Plan(No.GX2247)the Outstanding Chinese and Foreign Youth Exchange Program of China Association for Science and Technology(CAST)in 2019the Opening Project of Shanxi Key Laboratory of Advanced Manufacturing Technology(No.XJZZ202001)the Scientific Research Project of Shaanxi Education Department(No.20JS108)Open Foundation of Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and Technology(No.KFKT2021-01)Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry and Technology,Shaanxi University of Science and Technology(No.KFKT2021-01).
文摘Greenhouse gas emissions from waste plastics have caused global warming all over the world,which has been a central threat to the ecological environment for humans,flora and fauna.Among waste plastics,waste polyethylene terephthalate(PET)is attractive due to its excellent stability and degradation-resistant.Therefore,merging China’s carbon peak and carbon neutrality goals would be beneficial.In this review,we summarize the current state-of-the-art of carbon emission decrease from a multi-scale perspective technologically.We suggest that the carbon peak for waste PET can be achieved by employing the closed-loop supply chain,including recycling,biomass utilization,carbon capture and utilization.Waste PET can be a valuable and renewable resource in the whole life cycle.Undoubtedly,all kinds of PET plastics can be ultimately converted into CO_(2),which can also be feedstock for various kinds of chemical products,including ethyl alcohol,formic acid,soda ash,PU,starch and so on.As a result,the closed-loop supply chain can help the PET plastics industry drastically reduce its carbon footprint.
基金supported by the State Key Laboratory of Advanced Metallurgy,China(Project Code:41603006).
文摘Decarbonization is a critical issue for peaking CO_(2) emissions of energy-intensive industries,such as the iron and steel industry.The decarbonization options of China’s ironmaking and steelmaking sector were discussed based on a systematic three-dimensional low-carbon analysis from the aspects of resource utilization(Y),energy utilization(Q),and energy cleanliness which is evaluated by a process general emission factor(PGEF)on all the related processes,including the current blast furnace(BF)-basic oxygen furnace(BOF)integrated process and the specific sub-processes,as well as the electric arc furnace(EAF)process,typical direct reduction(DR)process,and smelting reduction(SR)process.The study indicates that the three-dimensional aspects,particularly the energy structure,should be comprehensively considered to quantitatively evaluate the decarbonization road map based on novel technologies or processes.Promoting scrap utilization(improvement of Y)and the substitution of carbon-based energy(improvement of PGEF)in particular is critical.In terms of process scale,promoting the development of the scrap-based EAF or DR-EAF process is highly encouraged because of their lower PGEF.The three-dimensional method is expected to extend to other processes or industries,such as the cement production and thermal electricity generation industries.
基金supported by the Fundamental Research Funds for the Central Universities of Southwest Jiaotong University,supported by Sichuan Science and Technology Program(2021YFS0284).
文摘Hydrothermal carbonization is highly applicable to high moisture biomass upgrading due to the fact that moist-ure involved can be directly used as reaction media under the subcritical-water region.With this,value-added utilization of hydrochar as solid fuel with high carbon and energy density is one of the important pathways for biomass conversion.In this review,the dewatering properties of hydrochar after the hydrothermal carbonization of biowaste,coalification degree with elemental composition and evolution,pelletization of hydrochar to enhance the mechanical properties and density,coupled with the combustion properties of hydrochar biofuel were discussed with various biomass and carbonization parameters.Potential applications for the co-combustion with coal,cleaner properties and energy balance for biowaste hydrothermal carbonization were presented as well as the challenges.
文摘High-performance carbonaceous electrode materials for supercapacitors were synthesized by subjecting corn starch to a simple molten salt activation process with K<sub>2</sub>CO<sub>3</sub> at a temperature of 850˚C. The resulting carbon material, obtained after activating for 1 hour, displayed excellent capacitive properties due to the synergistic effects of its porous structure. Utilizing these electrodes, the supercapacitor exhibited a high discharge capacitance (248 F g<sup>−1</sup> at 1 A g<sup>−1</sup>), which is 2.4 times higher than that of activated carbon without K<sub>2</sub>CO<sub>3</sub> activation. The enhancement in electrical performance was analyzed through SEM and XRD analysis, revealing that the porous and disordered structure provides a greater number of charge storage sites, resulting in improved capacitive performance.
文摘湖泊沉积物不仅记录了湖泊演化的过程,还蕴含了丰富的碳储量。本文以青藏高原西部郭扎错407 cm长的湖芯为例,探讨了8.7 ka BP以来该湖由淡水湖演变到咸水湖的过程中,有机碳和无机碳沉积通量与储量的变化及影响因素。郭扎错无机碳沉积通量范围为4.6~35.1 g·m^(-2)·a^(-1),平均值为17 g·m^(-2)·a^(-1),无机碳储量范围为2.5×10^(6)~19.1×10^(6) t/a,平均值为9.2×10^(6) t/a,无机碳总储量约为18.5×10^(9) t。有机碳沉积通量范围为1.6~7.3 g·m^(-2)·a^(-1),平均值为4.0 g·m^(-2)·a^(-1),有机碳储量范围为1.5×10^(6)~3.3×10^(6) t/a,平均值为2.2×10^(6) t/a,有机碳总储量约为1.63×10^(9) t。8.7 ka BP以来,三个不同环境演化阶段(8.7~4.0 ka BP,4.0~1.5 ka BP,以及1.5 ka BP至今)中,4.0~1.5 ka BP气候寒冷干旱,湖泊为淡水湖,但无机碳和有机碳的沉积通量和储量都表现为低值。根据碳沉积通量和储量的变化特征发现,无机碳的沉积与碳酸盐矿物成因有关,而有机碳沉积则与黏土矿物的成因有关,二者都与环境、湖水性质变化有关,其中温度对无机碳沉积通量和储量的影响大于盐度的影响,而温度对有机碳沉积通量和储量的影响小于盐度的影响。